Aerosolization of soil-dust and organic aggregates in sea spray facilitates the long-range transport of bacteria, and likely viruses across the free atmosphere. Although long-distance transport occurs, there are many uncertainties associated with their deposition rates. Here, we demonstrate that even in pristine environments, above the atmospheric boundary layer, the downward flux of viruses ranged from 0.26 × 10 to >7 × 10 m per day. These deposition rates were 9-461 times greater than the rates for bacteria, which ranged from 0.3 × 10 to >8 × 10 m per day. The highest relative deposition rates for viruses were associated with atmospheric transport from marine rather than terrestrial sources. Deposition rates of bacteria were significantly higher during rain events and Saharan dust intrusions, whereas, rainfall did not significantly influence virus deposition. Virus deposition rates were positively correlated with organic aerosols <0.7 μm, whereas, bacteria were primarily associated with organic aerosols >0.7 μm, implying that viruses could have longer residence times in the atmosphere and, consequently, will be dispersed further. These results provide an explanation for enigmatic observations that viruses with very high genetic identity can be found in very distant and different environments.

Remote lakes are usually unaffected by direct human influence, yet they receive inputs of atmospheric pollutants, dust, and other aerosols, both inorganic and organic. In remote, alpine lakes, these atmospheric inputs may influence the pool of dissolved organic matter, a critical constituent for the biogeochemical functioning of aquatic ecosystems. Here, to assess this influence, we evaluate factors related to aerosol deposition, climate, catchment properties, and microbial constituents in a global dataset of 86 alpine and polar lakes. We show significant latitudinal trends in dissolved organic matter quantity and quality, and uncover new evidence that this geographic pattern is influenced by dust deposition, flux of incident ultraviolet radiation, and bacterial processing. Our results suggest that changes in land use and climate that result in increasing dust flux, ultraviolet radiation, and air temperature may act to shift the optical quality of dissolved organic matter in clear, alpine lakes.

Iron (Fe) and dissolved organic matter (DOM) cycling have been implicated in arsenic mobilization via microbially mediated Fe oxide reduction. To evaluate the sources and multiple roles of DOM in Bangladesh aquifers, we conducted spectroscopic analyses on various types of surface water and groundwater samples from a site representative of aquifer chemistry and hydrology. Surface water contained humic substances with oxidized quinone-like moieties and high concentrations of labile microbially derived DOM. In contrast, in shallow groundwater where dissolved iron and arsenic concentrations were high, the quinone-like moieties of humic substances were more reduced, with less abundant labile DOM than that of surface water. Instead, DOM at these depths was characterized by terrestrial (plant/soil) signatures. A sediment microcosm experiment demonstrated that Fe(II) and terrestrially derived DOM were released from sediment over time. The results provide new evidence to support a dual role of natural DOM in Bangladesh aquifers (1) as a labile substrate for Fe- and humic-reducing bacteria and (2) as an electron shuttle via humic substances to enhance microbial iron reduction. Fluorescence index, amino acid-like fluorescence, and redox index may serve as useful indicators of the type of DOM likely to be involved in Fe solubilization and potentially As mobilization reactions.

Abstract. Many alpine areas are experiencing deglaciation, biogeochemical changes driven by temperature rise, and changes in atmospheric deposition. There is mounting evidence that the water quality of alpine streams may be related to these changes, including rising atmospheric deposition of carbon (C) and nutrients. Given that barren alpine soils can be severely C limited, atmospheric deposition sources may be an important source of C and nutrients for these environments. We evaluated the magnitude of atmospheric deposition of C and nutrients to an alpine site, the Green Lake 4 catchment in the Colorado Rocky Mountains. Using a long-term dataset (2002)(2003)(2004)(2005)(2006)(2007)(2008)(2009)(2010) of weekly atmospheric wet deposition and snowpack chemistry, we found that volume weighted mean dissolved organic carbon (DOC) concentrations were 1.12 ± 0.19 mg l −1 , and weekly concentrations reached peaks as high at 6-10 mg l −1 every summer. Total dissolved nitrogen concentration also peaked in the summer, whereas total dissolved phosphorus and calcium concentrations were highest in the spring. To investigate potential sources of C in atmospheric deposition, we evaluated the chemical quality of dissolved organic matter (DOM) and relationships between DOM and other solutes in wet deposition. Relationships between DOC concentration, fluorescence, and nitrate and sulfate concentrations suggest that pollutants from nearby urban and agricultural sources and organic aerosols derived from sub-alpine vegetation may influence high summer DOC wet deposition concentrations. Interestingly, high DOC concentrations were also recorded during "dust-in-snow" events in the spring, which may reflect an association of DOM with dust. Detailed chemical and spectroscopic analyses conducted for samples collected in 2010 revealed that the DOM in many late spring and summer samples was less aromatic and polydisperse and of lower molecular weight than that of winter and fall samples. Our C budget estimates for the Green Lake 4 catchment illustrated that wet deposition (9.9 kg C ha −1 yr −1 ) and dry deposition (6.9 kg C ha −1 yr −1 ) were a combined input of approximately 17 kg C ha −1 yr −1 , which could be as high as 24 kg C ha −1 yr −1 in high dust years. This atmospheric C input approached the C input from microbial autotrophic production in barren soils. Atmospheric wet and dry deposition also contributed 4.3 kg N ha −1 yr −1 , 0.15 kg P ha −1 yr −1 , and 2.7 kg Ca 2+ ha −1 yr −1 to this alpine catchment.

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The abundant thaw lakes and ponds in the circumarctic receive a new pool of organic carbon as permafrost peat soils degrade, which can be exposed to significant irradiance that potentially increases as climate warms and ice cover shortens. Exposure to sunlight is known to accelerate the transformation of dissolved organic matter (DOM) into molecules that can be more readily used by microbes. We sampled the water from two common classes of ponds found in the ice-wedge system of continuous permafrost regions of Canada, polygonal and runnel ponds, and followed the transformation of DOM over 12 days by looking at dissolved organic carbon (DOC) concentration and DOM absorption and fluorescence properties. The results indicate a relatively fast decay of color (3.4 and 1.6% loss d −1 of absorption at 320 nm for the polygonal and runnel pond, respectively) and fluorescence (6.1 and 8.3% loss d −1 of total fluorescent components, respectively) at the pond surface, faster in the case of humic-like components, but insignificant losses of DOC over the observed period. This result indicates that direct DOM mineralization (photochemical production of CO 2 ) is apparently minor in thaw ponds compared to the photochemical transformation of DOM into less chromophoric and likely more labile molecules with a greater potential for microbial mineralization. Therefore, DOM photolysis in arctic thaw ponds can be considered as a catalytic mechanism, accelerating the microbial turnover of mobilized organic matter from thawing permafrost and the production of greenhouse gases, especially in the most shallow ponds. Under a warming climate, this mechanism will intensify as summers lengthen.

In some high As groundwater systems, correlations are observed between dissolved organic matter (DOM) and As concentrations, but in other systems such relationships are not observed. The role of labile DOM as the main driver of microbial reductive dissolution does not explain the variation in these relationships. Other processes that may also influence arsenic mobility include complexation of As by dissolved humic substances, and competitive sorption and electron shuttling reactions mediated by humics. To evaluate such humic interactions, we characterized the optical properties of whole waters sampled from groundwater, spanning an age gradient in Araihazar, Bangladesh. Further, we analyzed fulvic acids (FA) isolated from large volume samples for optical properties, C and N content and 13C-NMR spectroscopic distribution. Old groundwater (> 30 years old) contained primarily sediment-derived DOM and had significantly higher (p < 0.001) dissolved arsenic concentration than groundwater that was < 5 years old. Younger groundwater had DOM spectroscopic signatures similar to surface water DOM and characteristic of a sewage pollution influence. Associations between dissolved arsenic, iron, and FA concentration, and fluorescence properties of isolated FA suggest that aromatic, terrestrially-derived FAs promote arsenic-iron-FA complexation reactions that enhance arsenic mobility.

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